The ability to modify the giant magnetoimpedance (GMI) effect in amorphous glass-coated ferromagnetic Co-based microwire reinforced polymer via laser irradiation is presented. Through in-situ laser annealing of microwires embedded into a polymer matrix, a 25 % improvement in the GMI response is demonstrated after only 4.9 min of annealing. This improvement is compared to a conventional oven anneal technique, requiring an hour of oven annealing, subsequent sample cooling and polymer casting. This unique in-situ technique offers a novel and expedient path toward tailorable multi-functional composites in the areas of tunable electromagnetic shielding, structurally integrated antennas and magnetic sensors.